High-entropy tantalum-zirconium-carbon ceramic precursor and preparation method thereof

A controlled preparation method for high-entropy tantalum-zirconium-carbon ceramic precursors addresses the issues of low controllability and thermal stability in existing methods, achieving high yields and improved mechanical properties.

CN119080500APending Publication Date: 2024-12-06FUDAN UNIVERSITY
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Patent Information

Application Number
CN202411167013.8
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2024-08-23
Publication Date
2024-12-06

AI Technical Summary

Technical Problem

Existing methods for preparing high-entropy carbide ceramic precursors suffer from low controllability and poor thermal stability, resulting in low ceramic conversion rates and poor high-temperature mechanical properties.

Method used

A method involving the preparation of a high-entropy tantalum-zirconium-carbon ceramic precursor through a series of controlled reactions using specific metal ion coordinators, organic solvents, and heat treatments to form a stable ceramic precursor with improved mechanical properties.

Benefits of technology

The method achieves high ceramic yields and enhanced high-temperature mechanical properties, with bending strengths of 565-598 MPa at 900°C and 588-598 MPa at 1600°C, demonstrating improved thermal stability and controllability.

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Abstract

The invention provides a high-entropy tantalum-zirconium-carbon ceramic precursor and a preparation method thereof, and belongs to the technical field of ceramic materials, and the preparation method comprises the following steps: in a nitrogen atmosphere, adding a metal ion strong coordination agent into a tantalum source solution, carrying out heating reaction, adding a metal ion weak coordination agent, and carrying out heating reaction; then adding a mixture of an organic solvent and water, and sequentially carrying out heating reflux and curing to obtain a tantalum carbide ceramic precursor in a nitrogen atmosphere; preparing a zirconium intermediate 1; preparing a zirconium intermediate 2; under anhydrous and anaerobic conditions, uniformly stirring an organic solvent, the zirconium intermediate 1 and the zirconium intermediate 2, and reacting to obtain a zirconium carbide ceramic precursor; uniformly stirring the tantalum carbide ceramic precursor, the zirconium carbide ceramic precursor and an organic solvent, and sequentially carrying out heat treatment and drying to obtain the high-entropy tantalum-zirconium-carbon ceramic precursor. The high-entropy tantalum-zirconium-carbon ceramic precursor with stable high-temperature mechanical properties can be prepared, the process is simple, the controllable degree is high, and the ceramic yield is high.
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Description

Technical Field

[0001] The present invention relates to the technical field of ceramic materials, and in particular to a high-entropy tantalum-zirconium-carbon ceramic precursor and a preparation method thereof. Background Art

[0002] High entropy ceramics are ultra-high temperature ceramics with high melting point (greater than 3000°C), high hardness, better oxidation resistance, corrosion resistance and high temperature stability. They can be used in ultra-high temperature environments (above 2000°C) and have very broad application prospects in aerospace, mechanical processing and other fields. There are many types of high entropy ceramic precursors, such as carbide high entropy ceramic precursors, boride high entropy ceramic precursors, nitride high entropy ceramic precursors, etc. Among them, the carbide molecules in the carbide high entropy ceramic precursors are easy to form a high entropy state, which is a good material for making high entropy ceramic precursors.

[0003] The existing single-component carbide ceramic precursors have the advantages of higher hardness, better oxidation resistance, etc. due to the high entropy effect, hysteresis diffusion effect and lattice distortion effect. At present, there are many methods for preparing high entropy composite carbide ceramic precursor materials, including carbon thermal reduction method, molten salt method, high temperature sintering method, SPS direct sintering method and high pressure sintering method. These methods have low controllability of the preparation process, and the obtained ceramic precursor materials have low ceramic conversion rate and poor thermal stability. Summary of the invention

[0004] In view of this, one of the purposes of the present invention is to overcome the shortcomings of the above-mentioned prior art and provide a method for preparing a high-entropy tantalum-zirconium-carbon ceramic precursor, which can prepare a high-entropy tantalum-zirconium-carbon ceramic precursor with stable high-temperature mechanical properties, and has a simple process, a high degree of controllability, and a high ceramic yield.

[0005] A second object of the present invention is to provide a high entropy tantalum-zirconium-carbon ceramic precursor.

[0006] In order to achieve one of the above purposes, the present invention adopts the following technical solutions:

[0007] A method for preparing a high entropy tantalum-zirconium-carbon ceramic precursor, the preparation method comprising the following steps:

[0008] Step S1, under a nitrogen atmosphere, adding a strong metal ion coordinator to a tantalum source solution, heating to 70-100° C. and mixing for 5-30 minutes, then adding a weak metal ion coordinator, and then adding a mixture of an organic solvent and water, heating to reflux and curing in sequence to obtain a tantalum carbide ceramic precursor;

[0009] In the step S1, the mass ratio of Ta, metal ion strong ligand, metal ion weak ligand, organic solvent and water in the tantalum source solution is 1:0.5-5:0.33-2:1-5:1;

[0010] Step S2, under a nitrogen atmosphere, stirring and dispersing zirconocene dichloride and an organic solvent, adding reagent 1 dropwise at a temperature of -10 to -5°C, heating to 0 to 50°C, reacting for 2 to 6 hours, filtering, and obtaining a zirconium intermediate 1;

[0011] In the step S2, the mass ratio of the zirconocene dichloride, the organic solvent and the reagent 1 is 4-30:10-86:1;

[0012] Step S3, at a temperature of -25 to -20°C, adding reagent 2 dropwise to zirconocene dichloride, introducing hydrogen, stirring for 2.2 to 5.8 hours, filtering, adding polyolefin to the filtrate, then heating to 78 to 82°C and reacting for 1.8 to 2.2 hours to obtain zirconium intermediate 2;

[0013] In the step S3, the mass ratio of zirconocene dichloride, reagent 2 and polyolefin is 4-30:1:2-10;

[0014] Step S4, under anhydrous and oxygen-free conditions, the organic solvent, zirconium intermediate 1 and zirconium intermediate 2 are uniformly stirred, reacted at a temperature of 58 to 62° C. for 3.8 to 4.2 hours, and then recovered to obtain a zirconium carbide ceramic precursor;

[0015] In the step S4, the mass ratio of the organic solvent, the zirconium intermediate 1 and the zirconium intermediate 2 is 3-60:1:1-10;

[0016] Step S5, stirring the tantalum carbide ceramic precursor, the zirconium carbide ceramic precursor and the organic solvent evenly, and then sequentially performing heat treatment and drying to obtain a high entropy tantalum zirconium carbon ceramic precursor.

[0017] In the step S5, the mass ratio of the tantalum carbide ceramic precursor, the zirconium carbide ceramic precursor and the organic solvent is 1-10:1:6-110.

[0018] Furthermore, in the step S1, the mass ratio of the mixture of Ta, the strong metal ion ligand, the weak metal ion ligand, the organic solvent and water in the tantalum source solution is 1:1.5-3:0.8-1.2:2-4:1.

[0019] Furthermore, in the step S1, the heating reflux temperature is 80 to 130° C., and the time is 1 to 6 hours.

[0020] Further, in the step S1, the tantalum source is one or more of propyl tantalate, isopropyl tantalate, butyl tantalate, and isobutyl tantalate;

[0021] The strong metal ion ligand is one or more of diethyl malonate, ethanolamine, propionylacetone, and acetylacetone;

[0022] The metal ion weak coordinating agent is one or more of methyl tert-butyl ether, ethylene glycol dimethyl ether, ethylene glycol methyl ether, and ethylene glycol diethyl ether;

[0023] In the step S1, step S2, step S4 and step S5, the organic solvent is one or more of benzene, toluene, dichloromethane, tetrahydrofuran, anhydrous ether, DMF, anhydrous methanol and anhydrous ethanol.

[0024] Furthermore, in step S2, the reagent 1 is one or more of formic acid, tetrahydrofuran, acetone, dichloromethane, chloroform, acetylacetone, chloroform, n-hexane, cyclohexane, acetonitrile, N,N-dimethylformamide, and N,N-dimethylacetamide.

[0025] Furthermore, in the step S2, the mass ratio of the zirconocene dichloride, the organic solvent and the reagent 1 is 10-20:30-60:1;

[0026] In the step S3, the mass ratio of the zirconocene dichloride, the reagent 2 and the polyolefin is 10-20:1:4-8.

[0027] Furthermore, in the step S3, the molecular weight of the polyolefin is 8000 to 40000, preferably 10000 to 20000.

[0028] Further, in step S3, the reagent 2 is one or more of methyl lithium, ethyl lithium, propyl lithium, isopropenyl magnesium bromide, n-butenyl magnesium bromide, isobutenyl magnesium bromide, n-pentenyl magnesium bromide, and isopentenyl magnesium bromide;

[0029] The polyolefin is one or more of polyethylene, polypropylene, poly-1-butene, poly-1-hexene, and poly-1-octene.

[0030] Furthermore, in step S5, the heat treatment is carried out at a temperature of 150 to 250° C. and for a time of 5 to 24 hours.

[0031] In order to achieve the second objective above, the present invention adopts the following technical solution:

[0032] A high entropy tantalum-zirconium-carbon ceramic precursor is prepared by the above-mentioned preparation method.

[0033] The beneficial effects of the present invention are:

[0034] The present invention obtains a tantalum carbide ceramic precursor by heating a tantalum source solution, a strong metal ion ligand and a weak metal ion ligand under the action of a mixture of an organic solvent and water; obtains a zirconium intermediate 1 by reacting zirconocene dichloride and a reagent 1 under the action of an organic solvent; obtains a zirconium intermediate 2 by using zirconocene dichloride, a reagent 2 and a polyolefin under the catalytic action of hydrogen; obtains a polymer zirconium carbide ceramic precursor by using the zirconium intermediate 1 and the zirconium intermediate 2 under the action of an organic solvent; finally, by heat treating the tantalum carbide ceramic precursor and the zirconium carbide ceramic precursor under the action of an organic solvent, the metal Zr element is used to replace the zirconium carbide ceramic precursor in the tantalum carbide ceramic precursor. Part of the Ta element realizes the change process of the fracture from intergranular fracture to cascading fracture in the formation process of the high-entropy tantalum-zirconium-carbon ceramic precursor material, ensures that the high-temperature performance of the high-entropy tantalum-zirconium-carbon ceramic precursor material increases instead of decreases, and effectively improves the high-temperature mechanical properties (i.e. thermal stability) of the high-entropy tantalum-zirconium-carbon ceramic precursor material; the process of the invention is simple, the controllable degree is high, and the ceramic yield is high. The ceramic yields at 1400°C and 1600°C are 45.19-46.84% and 38.35-39.59% respectively, and the bending strengths at 900°C and 1600°C are 565-586MPa and 588-598MPa respectively, which has good practical application value. DETAILED DESCRIPTION

[0035] The present invention will be further described with reference to specific implementation modes below.

[0036] Embodiment 1:

[0037] 1. Under nitrogen atmosphere, diethyl malonate was added to the propyl tantalate solution, stirred evenly at 70°C, and then methyl tert-butyl ether was added (the addition amount was 1 / 3 of the mass of the propyl tantalate solution. After the reaction was complete, a mixture of water and benzene was added drop by drop. After the addition was completed, it was refluxed at 80°C for 1h. After removing the solvent, it was solidified to obtain a tantalum carbide ceramic precursor. Among them, the mass ratio of Ta, diethyl malonate, methyl tert-butyl ether, benzene and water in the propyl tantalate solution was 1:0.5:0.33:1:1.

[0038] 2. Under the protection of nitrogen, in a 250 mL three-necked flask, zirconocene dichloride was stirred and dispersed in benzene, formic acid was slowly added dropwise at -10°C, then the temperature was raised to 0°C to react for 2 hours, and filtered to obtain zirconium intermediate 1. The mass ratio of zirconocene dichloride, benzene and formic acid was 4:10:1.

[0039] 3. Under the protection of nitrogen, at -25°C, in a 250mL three-necked flask, methyl lithium was dropped into dichloro zirconocene, hydrogen was introduced and stirred for 2.2 hours to complete the reaction, polyethylene with a molecular weight of 8000 was added after filtration, the temperature was raised to 78°C and the reaction was carried out for 1.8 hours, and tantalum intermediate 2 was obtained by adjusting the degree of polymerization. Among them, the mass ratio of dichloro zirconocene, methyl lithium and polyethylene was 4:1:2.

[0040] 4. Under anhydrous and oxygen-free conditions, add benzene, zirconium intermediate 1 and zirconium intermediate 2 into a 250 mL three-necked flask, react at 58°C for 3.8 hours, recover the solvent benzene, and obtain a zirconium carbide ceramic precursor. The mass ratio of benzene, zirconium intermediate 1 and zirconium intermediate 2 is 3:1:1.

[0041] 5. Add tantalum carbide ceramic precursor, titanium carbide ceramic precursor and benzene into a reactor and stir evenly to obtain a precursor solution. Heat treat the precursor solution at 150°C for 5 hours and dry to obtain a tantalum zirconium carbon ceramic precursor. The mass ratio of tantalum carbide ceramic precursor, zirconium carbide ceramic precursor and benzene is 1:1:6.

[0042] In an argon atmosphere, the tantalum zirconium carbon ceramic precursor prepared in this embodiment was cured and then subjected to cracking tests at 1400°C and 1600°C, respectively. The ceramic yields at 1400°C and 1600°C under these conditions were calculated to be 45.19% and 38.35%, respectively. The bending strengths of the tantalum zirconium carbon ceramic precursor prepared in this embodiment at 900°C and 1600°C were 565MPa and 588MPa, respectively.

[0043] Embodiment 2:

[0044] 1. In a nitrogen atmosphere, add ethanolamine to the isopropyl tantalate solution, stir evenly at 70°C, then add ethylene glycol dimethyl ether to react completely, then add a mixture of water and toluene drop by drop, reflux at 130°C for 6 hours after the addition is complete, remove the solvent, and solidify to obtain a tantalum carbide ceramic precursor. The mass ratio of Ta, ethanolamine, ethylene glycol dimethyl ether, toluene and water in the isopropyl tantalate solution is 1:5:2:5:1.

[0045] 2. Under the protection of nitrogen, in a 250 mL three-necked flask, zirconocene dichloride was stirred and dispersed in toluene, tetrahydrofuran was slowly added dropwise at -5°C, then the temperature was raised to 50°C to react for 6 hours, and filtered to obtain zirconium intermediate 1. The mass ratio of zirconocene dichloride, toluene and tetrahydrofuran was 30:86:1.

[0046] 3. Under the protection of nitrogen, at -20°C, in a 250mL three-necked flask, ethyl lithium was dropped into dichloro zirconocene, hydrogen was introduced and stirred for 5.8 hours to complete the reaction, and polypropylene with a molecular weight of 40,000 was added after filtration, and the temperature was raised to 82°C for reaction for 2.2 hours. By adjusting the degree of polymerization, tantalum intermediate 2 was obtained. The mass ratio of dichloro zirconocene, ethyl lithium and polypropylene was 30:1:10.

[0047] 4. Under anhydrous and oxygen-free conditions, toluene, zirconium intermediate 1 and zirconium intermediate 2 were added to a 250 mL three-necked flask, reacted at 62°C for 4.2 hours, and the solvent benzene was recovered to obtain a zirconium carbide ceramic precursor. The mass ratio of toluene, zirconium intermediate 1 and zirconium intermediate 2 was 60:1:10.

[0048] 5. Add tantalum carbide ceramic precursor, titanium carbide ceramic precursor and toluene into a reactor and stir evenly to obtain a precursor solution. Heat treat the precursor solution at 250°C for 24 hours and dry to obtain a tantalum zirconium carbon ceramic precursor. The mass ratio of tantalum carbide ceramic precursor, zirconium carbide ceramic precursor and toluene is 10:1:110.

[0049] In an argon atmosphere, the tantalum zirconium carbon ceramic precursor prepared in this embodiment was cured and then subjected to cracking tests at 1400°C and 1600°C, respectively. The ceramic yields at 1400°C and 1600°C under these conditions were calculated to be 46.84% and 39.48%, respectively. The bending strengths of the tantalum zirconium carbon ceramic precursor prepared in this embodiment at 900°C and 1600°C were 578MPa and 594MPa, respectively.

[0050] Embodiment 3:

[0051] 1. Under a nitrogen atmosphere, add propionylacetone to the butyl tantalate solution, stir evenly at 70°C, then add ethylene glycol methyl ether to react completely, then add a mixture of water and dichloromethane drop by drop, reflux at 100°C for 3h after the addition is completed, remove the solvent, and solidify to obtain a tantalum carbide ceramic precursor.

[0052] The mass ratio of Ta, propionylacetone, ethylene glycol methyl ether, dichloromethane and water in the butyl tantalate solution is 1:1.5:0.8:2:1.

[0053] 2. Under the protection of nitrogen, in a 250 mL three-necked flask, dichlorozirconocene was stirred and dispersed in dichloromethane, acetone was slowly added dropwise at -6°C, then the temperature was raised to 15°C and the reaction was continued for 3 hours, and then filtered to obtain zirconium intermediate 1. The mass ratio of dichlorozirconocene, dichloromethane and acetone was 10:30:1.

[0054] 3. Under the protection of nitrogen, at -22°C, in a 250mL three-necked flask, propyl lithium was dropped into dichloro zirconocene, hydrogen was introduced and stirred for 3.5 hours to complete the reaction, and poly 1-butene with a molecular weight of 10,000 was added after filtration, and the temperature was raised to 80°C for reaction for 2 hours. By adjusting the degree of polymerization, tantalum intermediate 2 was obtained. The mass ratio of dichloro zirconocene, propyl lithium and poly 1-butene was 10:1:4.

[0055] 4. Under anhydrous and oxygen-free conditions, add dichloromethane, zirconium intermediate 1 and zirconium intermediate 2 into a 250 mL three-necked flask, react at 60°C for 4 hours, recover the solvent benzene, and obtain a zirconium carbide ceramic precursor. The mass ratio of dichloromethane, zirconium intermediate 1 and zirconium intermediate 2 is 20:1:3.

[0056] 5. Add tantalum carbide ceramic precursor, titanium carbide ceramic precursor and dichloromethane into a reaction kettle and stir evenly to obtain a precursor solution. Heat treat the precursor solution at 200° C. for 16 hours and dry to obtain a tantalum zirconium carbon ceramic precursor.

[0057] Wherein, the mass ratio of tantalum carbide ceramic precursor, zirconium carbide ceramic precursor and dichloromethane is 4:1:30.

[0058] In an argon atmosphere, the tantalum zirconium carbon ceramic precursor prepared in this embodiment was cured and then subjected to cracking tests at 1400°C and 1600°C, respectively. The ceramic yields at 1400°C and 1600°C under these conditions were calculated to be 46.35% and 39.59%, respectively. The bending strengths of the tantalum zirconium carbon ceramic precursor prepared in this embodiment at 900°C and 1600°C were 580MPa and 597MPa, respectively.

[0059] Embodiment 4:

[0060] 1. Under a nitrogen atmosphere, add acetylacetone to the isobutyl tantalate solution, stir evenly at 70°C, then add ethylene glycol diethyl ether to react completely, then add a mixture of water and tetrahydrofuran drop by drop, reflux at 120°C for 5 hours after the addition is completed, remove the solvent, and solidify to obtain a tantalum carbide ceramic precursor.

[0061] The mass ratio of Ta, acetylacetone, ethylene glycol diethyl ether, tetrahydrofuran and water in the isobutyl tantalate solution is 1:3:1.2:3:1.

[0062] 2. Under the protection of nitrogen, in a 250 mL three-necked flask, dichlorocyclopentadienyl zirconate was stirred and dispersed in tetrahydrofuran, and dichloromethane was slowly added dropwise at -8°C, then the temperature was raised to 35°C to react for 5 hours, and filtered to obtain zirconium intermediate 1. The mass ratio of dichlorocyclopentadienyl zirconate, tetrahydrofuran and dichloromethane was 20:60:1.

[0063] 3. Under the protection of nitrogen, at -24°C, in a 250mL three-necked flask, isopropenylmagnesium bromide was dropped into dichlorozirconocene, hydrogen was introduced and stirred for 5 hours to complete the reaction, and poly-1-hexene with a molecular weight of 20,000 was added after filtration, and the temperature was raised to 80°C for reaction for 2 hours, and tantalum intermediate 2 was obtained by adjusting the degree of polymerization. Among them, the mass ratio of dichlorozirconocene, isopropenylmagnesium bromide and poly-1-hexene is 20:1:8.

[0064] 4. Under anhydrous and oxygen-free conditions, tetrahydrofuran, zirconium intermediate 1 and zirconium intermediate 2 were added to a 250 mL three-necked flask, reacted at 60°C for 4 hours, and the solvent benzene was recovered to obtain a zirconium carbide ceramic precursor. The mass ratio of tetrahydrofuran, zirconium intermediate 1 and zirconium intermediate 2 was 40:1:8.

[0065] 5. Add tantalum carbide ceramic precursor, titanium carbide ceramic precursor and tetrahydrofuran into a reactor and stir evenly to obtain a precursor solution. Heat treat the precursor solution at 230°C for 20 hours and dry to obtain a tantalum zirconium carbon ceramic precursor. The mass ratio of tantalum carbide ceramic precursor, zirconium carbide ceramic precursor and tetrahydrofuran is 8:1:90.

[0066] In an argon atmosphere, the tantalum zirconium carbon ceramic precursor prepared in this embodiment was cured and then subjected to cracking tests at 1400°C and 1600°C, respectively. The ceramic yields at 1400°C and 1600°C under these conditions were calculated to be 46.54% and 39.57%, respectively. The bending strengths of the tantalum zirconium carbon ceramic precursor prepared in this embodiment at 900°C and 1600°C were 586MPa and 598MPa, respectively.

[0067] The above examples are only used to illustrate the technical solution of the present invention rather than to limit it. Although the present invention has been described in detail with reference to the best embodiment, a person skilled in the art should understand that the technical solution of the present invention can still be modified or replaced by equivalents, and these modifications or equivalent replacements cannot cause the modified technical solution to deviate from the spirit and scope of the technical solution of the present invention.

Claims

1. A method for preparing a high entropy tantalum-zirconium-carbon ceramic precursor, characterized in that: The preparation method comprises the following steps: Step S1, under a nitrogen atmosphere, adding a strong metal ion coordinator to a tantalum source solution, heating to 70-100° C. and mixing for 5-30 minutes, then adding a weak metal ion coordinator, and then adding a mixture of an organic solvent and water, heating to reflux and curing in sequence to obtain a tantalum carbide ceramic precursor; In the step S1, the mass ratio of Ta, metal ion strong ligand, metal ion weak ligand, organic solvent and water in the tantalum source solution is 1:0.5-5:0.33-2:1-5:1; Step S2, under a nitrogen atmosphere, stirring and dispersing zirconocene dichloride and an organic solvent, adding reagent 1 dropwise at a temperature of -10 to -5°C, heating to 0 to 50°C, reacting for 2 to 6 hours, filtering, and obtaining a zirconium intermediate 1; In the step S2, the mass ratio of the zirconocene dichloride, the organic solvent and the reagent 1 is 4-30:10-86:1; Step S3, at a temperature of -25 to -20°C, adding reagent 2 dropwise to zirconocene dichloride, introducing hydrogen, stirring for 2.2 to 5.8 hours, filtering, adding polyolefin to the filtrate, then heating to 78 to 82°C and reacting for 1.8 to 2.2 hours to obtain zirconium intermediate 2; In the step S3, the mass ratio of zirconocene dichloride, reagent 2 and polyolefin is 4-30:1:2-10; Step S4, under anhydrous and oxygen-free conditions, the organic solvent, zirconium intermediate 1 and zirconium intermediate 2 are uniformly stirred, reacted at a temperature of 58 to 62° C. for 3.8 to 4.2 hours, and then recovered to obtain a zirconium carbide ceramic precursor; In the step S4, the mass ratio of the organic solvent, the zirconium intermediate 1 and the zirconium intermediate 2 is 3-60:1:1-10; Step S5, stirring the tantalum carbide ceramic precursor, the zirconium carbide ceramic precursor and the organic solvent evenly, and then sequentially performing heat treatment and drying to obtain a high entropy tantalum zirconium carbon ceramic precursor. In the step S5, the mass ratio of the tantalum carbide ceramic precursor, the zirconium carbide ceramic precursor and the organic solvent is 1-10:1:6-110.

2. The preparation method according to claim 1, characterized in that: In the step S1, the mass ratio of the mixture of Ta, the strong metal ion coordinator, the weak metal ion coordinator, the organic solvent and water in the tantalum source solution is 1:1.5-3:0.8-1.2:2-4:

1.

3. The preparation method according to claim 2, characterized in that: In the step S1, the heating reflux temperature is 80-130° C. and the time is 1-6 hours.

4. The preparation method according to claim 3, characterized in that: In the step S1, the tantalum source is one or more of propyl tantalate, isopropyl tantalate, butyl tantalate, and isobutyl tantalate; The strong metal ion ligand is one or more of diethyl malonate, ethanolamine, propionylacetone, and acetylacetone; The metal ion weak coordinating agent is one or more of methyl tert-butyl ether, ethylene glycol dimethyl ether, ethylene glycol methyl ether, and ethylene glycol diethyl ether; In the step S1, step S2, step S4 and step S5, the organic solvent is one or more of benzene, toluene, dichloromethane, tetrahydrofuran, anhydrous ether, DMF, anhydrous methanol and anhydrous ethanol.

5. The preparation method according to any one of claims 1 to 4, characterized in that: In step S2, the reagent 1 is one or more of formic acid, tetrahydrofuran, acetone, dichloromethane, chloroform, acetylacetone, chloroform, n-hexane, cyclohexane, acetonitrile, N,N-dimethylformamide, and N,N-dimethylacetamide.

6. The preparation method according to claim 5, characterized in that: In the step S2, the mass ratio of the zirconocene dichloride, the organic solvent and the reagent 1 is 10-20:30-60:1; In the step S3, the mass ratio of the zirconocene dichloride, the reagent 2 and the polyolefin is 10-20:1:4-8.

7. The preparation method according to claim 6, characterized in that: In the step S3, the molecular weight of the polyolefin is 8000-40000, preferably 10000-20000.

8. The preparation method according to claim 7, characterized in that: In step S3, the reagent 2 is one or more of methyl lithium, ethyl lithium, propyl lithium, isopropenyl magnesium bromide, n-butenyl magnesium bromide, isobutenyl magnesium bromide, n-pentenyl magnesium bromide, and isopentenyl magnesium bromide; The polyolefin is one or more of polyethylene, polypropylene, poly-1-butene, poly-1-hexene, and poly-1-octene.

9. The preparation method according to claim 1, characterized in that: In the step S5, the heat treatment is performed at a temperature of 150 to 250°C for a time of 5 to 24 hours.

10. A high entropy tantalum-zirconium-carbon ceramic precursor, characterized in that: The high entropy tantalum-zirconium-carbon ceramic precursor is prepared by the preparation method described in any one of claims 1 to 10.